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Halide-free carbonylation of methanol with H-MOR supported CuCeO

Chaoli Tong, Jiachang Zuo, Danlu Wen, Weikun Chen, Linmin Ye, Youzhu Yuan

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1075-1087 doi: 10.1007/s11705-020-2019-5

摘要： Heterogeneous halide-free carbonylation of methanol to acetates, including methyl acetate (MA) and acetic acid, using non-precious metal catalysts has been a topic of interest for decades. The key issue is that the water produced by methanol dehydration inhibits the formation of acetyl species and reduces the MA selectivity. Here, we report that CuCeO /H-mordenite (H-MOR) catalyst can nearly eliminate the inhibiting effect of water on carbonylation by a water-gas shift reaction (WGSR) on-site, and can thus achieve 96.5% methanol conversion with 87.4% MA selectivity for the halide-free carbonylation of methanol. The results of powder X-ray diffraction, transmission electron microscopy, and scanning electron microscopy show that the Cu and Ce species are highly dispersed on H-MOR even when the CuCeO contents are as high as 29 wt-%. Fourier transform infrared spectroscopy and CO chemisorption analysis reveal that a small portion of Cu species can migrate into the channel of H-MOR when CuCeO /H-MOR is calcined at 500 °C and these Cu species are converted into Cu sites upon reduction. The Cu sites facilitate the WGSR and are also active sites for methanol carbonylation. The introduction of Ce benefits the inhibition of coke deposits and thus enhances the catalyst stability.

关键词： methanol carbonylation     halide-free     methyl acetate     H-mordenite     copper and cerium oxide    

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High performance solid-state thermoelectric energy conversion via inorganic metal halide perovskites

Lifu YAN, Lingling ZHAO, Guiting YANG, Shichao LIU, Yang LIU, Shangchao LIN

《能源前沿（英文）》 2022年 第16卷 第4期   页码 581-594 doi: 10.1007/s11708-022-0831-y

摘要： Solid-state thermoelectric energy conversion devices attract broad research interests because of their great promises in waste heat recycling, space power generation, deep water power generation, and temperature control, but the search for essential thermoelectric materials with high performance still remains a great challenge. As an emerging low cost, solution-processed thermoelectric material, inorganic metal halide perovskites CsPb(I1–xBrx)3 under mechanical deformation is systematically investigated using the first-principle calculations and the Boltzmann transport theory. It is demonstrated that halogen mixing and mechanical deformation are efficient methods to tailor electronic structures and charge transport properties in CsPb(I1–xBrx)3 synergistically. Halogen mixing leads to band splitting and anisotropic charge transport due to symmetry-breaking-induced intrinsic strains. Such band splitting reconstructs the band edge and can decrease the charge carrier effective mass, leading to excellent charge transport properties. Mechanical deformation can further push the orbital energies apart from each other in a more controllable manner, surpassing the impact from intrinsic strains. Both anisotropic charge transport properties andZT values are sensitive to the direction and magnitude of strain, showing a wide range of variation from 20% to 400% (with a ZT value of up to 1.85) compared with unstrained cases. The power generation efficiency of the thermoelectric device can reach as high as approximately 12% using mixed halide perovskites under tailored mechanical deformation when the heat-source is at 500 K and the cold side is maintained at 300 K, surpassing the performance of many existing bulk thermoelectric materials.

关键词： inorganic metal halide perovskites     mechanical deformation     thermoelectrics     first-principle calculations     Boltzmann transport theory    

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Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots

Yonghyun Kim, Huiwen Liu, Yi Liu, Boa Jin, Hao Zhang, Wenjing Tian, Chan Im

《化学科学与工程前沿（英文）》 2021年 第15卷 第1期   页码 187-197 doi: 10.1007/s11705-020-1931-z

摘要： Cesium lead halide perovskite (CsPbX , X= Cl, Br, I) quantum dots (QDs) and their partly Mn -substituted QDs (CsPb Mn X ) attract considerable attention owing to their unique photoluminescence (PL) efficiencies. The two types of QDs, having different PL decay dynamics, needed to be further investigated in a form of aggregates to understand their solid-state-induced exciton dynamics in conjunction with their behaviors upon degradation to achieve practical applications of those promising QDs. However, thus far, these QDs have not been sufficiently investigated to obtain deep insights related to the long-term stability of their PL properties as aggregated solid-states. Therefore, in this study, we comparatively examined CsPbX - and CsPb Mn X -type QDs stocked for>50 d under dark ambient conditions by using excitation wavelength-dependent PL quantum yield and time-resolved PL spectroscopy. These investigations were performed with powder samples in addition to solutions to determine the influence of the inter-QD interaction of the aged QD aggregates on their radiative decays. It turns out that the Mn -substituted QDs exhibited long-lasting PL quantum efficiencies, while the unsubstituted CsPbX -type QDs exhibited a drastic reduction of their PL efficiencies. And the obtained PL traces were clearly sensitive to the sample status. This is discussed with the possible interaction depending on the size and distance of the QD aggregates.

关键词： quantum dots     cesium lead halide perovskite     time-resolved photoluminescence     PL quantum yield     QD aggregates    

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Cell-free systems in the new age of synthetic biology

Fernando Villarreal,Cheemeng Tan

《化学科学与工程前沿（英文）》 2017年 第11卷 第1期   页码 58-65 doi: 10.1007/s11705-017-1610-x

摘要： The advent of synthetic biology has ushered in new applications of cell-free transcription-translation systems. These cell-free systems are reconstituted using cellular proteins, and are amenable to modular control of their composition. Here, we discuss the historical advancement of cell-free systems, as well as their new applications in the rapid design of synthetic genetic circuits and components, directed evolution of biomolecules, diagnosis of infectious diseases, and synthesis of vaccines. Finally, we present our vision on the future direction of cell-free synthetic biology.

关键词： cell-free system     application    

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Recent advances in cycloaddition of CO with epoxides: halogen-free catalysis and mechanistic insights

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1879-1894 doi: 10.1007/s11705-023-2354-4

摘要： The atom-economical cycloaddition of CO2 with epoxides to synthesize cyclic carbonates is a promising route for valuable utilization of CO2. Halogenide such as alkali metal halides and quaternary ammonium salt have been developed as the efficient catalysts. However, the spilled halogen causes equipment corrosion and affects the product purity. To address these concerns, the halogen-free cycloaddition of CO2 with epoxides has always been desired. In this review, we systematically discussed the halogen-free catalysis for cycloaddition of CO2 with epoxides from the mechanistic insights, aiming to promote the development of efficient halogen-free catalysts. Two types of catalysts, i.e., alternatives of halogen nucleophiles for epoxide activation, and bifunctional catalysts with Lewis acid-base sites for synergistic activation of CO2 and epoxides are summarized and emphasized. Specially, metal oxides as the potential halogen-free catalysts are highlighted due to their flexible acid-base sites for synergistic activation of CO2 and epoxides, facile preparation, and low cost.

关键词： carbon dioxide     halogen-free catalysis     cyclic carbonate     mechanistic insight    

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Hollow carbon spheres and their noble metal-free hybrids in catalysis

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1380-1407 doi: 10.1007/s11705-021-2097-z

摘要： Hollow carbon spheres have garnered great interest owing to their high surface area, large surface-to-volume ratio and reduced transmission lengths. Herein, we overview hollow carbon sphere-based materials and their noble metal-free hybrids in catalysis. Firstly, we summarize the key fabrication techniques for various kinds of hollow carbon spheres, with a particular emphasis on controlling pore structure and surface morphology, and then heterogeneous doping as well as their metal-free/containing hybrids are presented; next, possible applications for non-noble metal/hollow carbon sphere hybrids in the area of energy-related catalysis, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, water splitting, rechargeable Zn-air batteries and pollutant degradation are discussed; finally, we introduce the various challenges and opportunities offered by hollow carbon spheres from the perspective of synthesis and catalysis.

关键词： hollow carbon spheres     functionalization     noble metal-free     catalysis    

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Decontamination of Cr(VI) facilitated formation of persistent free radicals on rice husk derived biochar

Kaikai Zhang, Peng Sun, Yanrong Zhang

《环境科学与工程前沿（英文）》 2019年 第13卷 第2期 doi: 10.1007/s11783-019-1106-7

摘要：

PFRs were produced on biochar during Cr(VI) decontamination.

PFRs formation on biochar was owing to the oxidization of phenolic-OH by Cr(VI).

Appearance of excessive oxidant led to the consumption of PFRs on biochar.

Biochar charred at high temperature possessed great performance to Cr(VI) removal.

关键词： Biochar     Persistent free radicals     Phenolic hydroxyl groups     Cr(VI) reduction    

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Thermoresponsive block copolymer supported Pt nanocatalysts for base-free aerobic oxidation of 5-hydroxymethyl

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1514-1523 doi: 10.1007/s11705-021-2092-4

摘要： A base-free catalytic system for the aerobic oxidation of 5-hydroxymethyl-2-furfural was exploited by using Pt nanoparticles immobilized onto a thermoresponsive poly(acrylamide-co-acrylonitrile)-b-poly(N-vinylimidazole) block copolymer, with an upper critical solution temperature of about 45 °C. The Pt nanocatalysts were well-dispersed and highly active for the base-free oxidation of 5-hydroxymethyl-2-furfural by molecular oxygen in water, affording high yields of 2,5-furandicarboxylic acid (up to>99.9%). The imidazole groups in the block copolymer were conducive to the improvement of catalytic performance. Moreover, the catalysts could be easily separated and recovered based on their thermosensitivity by cooling the reaction system below the upper critical solution temperature. Good stability and reusability were observed over these copolymer-immobilized catalysts with no obvious decrease in catalytic activity in the five consecutive cycles.

关键词： aerobic oxidation     base-free     5-hydroxymethyl-2-furfural     Pt nanoparticle     thermoresponsive block copolymer    

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Influence of the filler materials on flux-free brazing of pure aluminium (1050)

Kirsten BOBZIN, Lidong ZHAO, Thomas SCHLAEFER, Thomas WARDA,

《机械工程前沿（英文）》 2010年 第5卷 第1期   页码 47-51 doi: 10.1007/s11465-009-0079-9

摘要： In the present study, samples of pure aluminium (1050) were deposited by cold spraying with filler materials such as Al12Si, Al7Si, Al12Si-4%Cu, and the Al-Si-based filler material A, which was especially developed for flux-free brazing by the Surface Engineering Institute. Besides, pure Si powder was also sprayed. The coated samples were heat-treated under different conditions and were brazed under an argon atmosphere without fluxes or with the flux Nokolok by an induction heating system. The shear strength of the brazed joints was determined. The results show that the filler materials could be well deposited by cold spraying. A thin layer of brittle Si could also form due to the strong deformation of the substrate surface. The heat treatments showed that a very good metallurgical bond between the filler materials and the substrate could be realized by the deposition by cold spraying. The Al7Si deposited samples could not be brazed without fluxes under the given conditions. The samples deposited with other filler materials could be brazed without fluxes. The in-situ diffusion process made it possible to braze the Si-deposited samples at 580°C. The joints of the samples deposited with the filler material showed the highest shear strength of 41 MPa, whereas the values of the Al12Si and Si deposited samples were less than 20 MPa. The employment of the flux Nikolok significantly increased the shear strength of the Al12Si deposited samples to more than 53 MPa.

关键词： aluminium     flux-free brazing     cold spraying     shear strength    

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New perspectives in free nitrous acid (FNA) uses for sustainable wastewater management

《环境科学与工程前沿（英文）》 2023年 第18卷 第2期 doi: 10.1007/s11783-024-1786-5

摘要：

● The historical development of free nitrous acid (FNA) technologies is reviewed.

关键词： Free nitrous acid     Acid-tolerant ammonia oxidizer     In situ generation     Wastewater management    

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Highly selective detection of copper(II) by a “ligand-free” conjugated copolymer in nucleophilic solvents

Weixing Deng, Pengfei Sun, Quli Fan, Lei Zhang, Tsuyoshi Minami

《化学科学与工程前沿（英文）》 2020年 第14卷 第1期   页码 105-111 doi: 10.1007/s11705-019-1791-6

摘要： The synthesis of -cyclohexyl carbamate-attached fluorene- -phenylene copolymer (PFPNCC) and the use of PFPNCC as a “ligand-free” fluorescent chemosensor for Cu(II) are described. Addition of Cu(II) can efficiently quench the fluorescence of PFPNCC in nucleophilic solvents such as DMF and DMSO, but not in low nucleophilic solvents such as 1,4-dioxane and THF. Ultraviolet-visible spectra of the mixture of the conjugated polymer and Cu(II) indicate the presence of a reduced Cu(I) ion in the solution. Furthermore, fluorescence recovery of PFPNCC observed at low temperature suggests that the quenching and reducing mechanism is most probably due to a photo-induced electron transfer from excited PFPNCC to Cu(II). Our findings provide a novel strategy for highly selective conjugated polymer-based chemosensors for various target analytes, albeit “ligand-free”.

关键词： ligand-free     fluorescent chemosensor     copper     photo-induced electron transfer    

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Ionically Imprinting-Based Copper (Ⅱ) Label-Free Detection for Preventing Hearing Loss Article

Huan Wang, Hui Zhang, Xiaoli Zhang, Hong Chen, Ling Lu, Renjie Chai

《工程（英文）》 doi: 10.1016/j.eng.2023.09.001

摘要：

Copper is a microelement with important physiological functions in the body. However, the excess copper ion (Cu2+) may cause severe health problems, such as hair cell apoptosis and the resultant hearing loss. Therefore, the assay of Cu2+ is important. We integrate ionic imprinting technology (IIT) and structurally colored hydrogel beads to prepare chitosan-based ionically imprinted hydrogel beads (IIHBs) as a low-cost and high-specificity platform for Cu2+ detection. The IIHBs have a macroporous microstructure, uniform size, vivid structural color, and magnetic responsiveness. When incubated in solution, IIHBs recognize Cu2+ and exhibit a reflective peak change, thereby achieving label-free detection. In addition, benefiting from the IIT, the IIHBs display good specificity and selectivity and have an imprinting factor of 19.14 at 100 lmol∙L–1. These features indicated that the developed IIHBs are promising candidates for Cu2+ detection, particularly for the prevention of hearing loss.

关键词： Structural color     Microfluidics Ionic imprinting     Label-free detection     Hearing loss    

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Solvent-free mechanochemical mild oxidation method to enhance adsorption properties of chitosan

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1416-4

摘要：

• Solvent-free chitosan oxidation is obtained by rapid mechanochemical reaction.

关键词： Chitosan     High energy ball milling     Mechanochemistry     Oxidation    

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Design approach for single piston hydraulic free piston diesel engines

Wei WU, Shihua YUAN, Jibin HU, Chongbo JING,

《机械工程前沿（英文）》 2009年 第4卷 第4期   页码 371-378 doi: 10.1007/s11465-009-0069-y

摘要： The operating characteristics of a single piston hydraulic free piston diesel engine differ significantly from conventional diesel engines and this provides a theoretical basis for controlling and optimizing the design of the engine. The design of the proposed engine intended as a power supply for a hydraulic propulsion vehicle is presented. An engine performance forecast model was generated in AMESim. The performance of the prototype engine is predicted and the predictive results are verified with experiments. The particular features of the engine are discussed. The dynamic characteristics of the prototype engine are analyzed and the results indicate the rationality and feasibility of the engine design parameters. The features of the controllable working frequency and the intermittence output flows are provided. The flow capacity characteristics of the hydraulic valves on the prototype engine are offered. The methods for starting and the operation after misfire are presented.

关键词： free piston engine (FPE)     diesel engine     hydraulic equipment     simulation     experiment    

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“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 207-212 doi: 10.1007/s11705-009-0240-3

摘要： With the rapid expansion of the global motor vehicle population, the transportation sector has taken up a growing proportion among all the carbon dioxide emission-related sectors. To contribute to solutions of the carbon dioxide-oriented problem in transportation, this paper proposes the “ALL FREE” concept that applies partial oxidation process instead of the conventional complete oxidation to vehicle engines. In such an engine, the fuels are partially oxidized into corresponding chemical products, which, as a result, enable the process to be theoretically free of CO, while the heat output of the partial oxidation could drive the vehicle. On the other hand, the resulting products are of great value, which could decrease or even counteract the cost of fuels in transportation. In this paper, the thermodynamic and kinetic data (e.g., the heat output and heat release rate) of five selected partial oxidation reactions were calculated at length to demonstrate and exemplify the theoretical feasibility of the “ALL FREE” concept. It turned out that the partial oxidation of -butane to maleic anhydride has the most potential to meet the basic requirements of this concept. To sum up, this design concept is of significant application potential for the reduction of CO emissions in the transportation industry, although there remain many technical challenges.

关键词： oxidation process     CO     complete oxidation     ALL FREE     -butane    

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标题 作者 时间 类型 操作

Halide-free carbonylation of methanol with H-MOR supported CuCeO

Chaoli Tong, Jiachang Zuo, Danlu Wen, Weikun Chen, Linmin Ye, Youzhu Yuan

期刊论文

High performance solid-state thermoelectric energy conversion via inorganic metal halide perovskites

Lifu YAN, Lingling ZHAO, Guiting YANG, Shichao LIU, Yang LIU, Shangchao LIN

期刊论文

Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots

Yonghyun Kim, Huiwen Liu, Yi Liu, Boa Jin, Hao Zhang, Wenjing Tian, Chan Im

期刊论文

Cell-free systems in the new age of synthetic biology

Fernando Villarreal,Cheemeng Tan

期刊论文

Recent advances in cycloaddition of CO with epoxides: halogen-free catalysis and mechanistic insights

期刊论文

Hollow carbon spheres and their noble metal-free hybrids in catalysis

期刊论文

Decontamination of Cr(VI) facilitated formation of persistent free radicals on rice husk derived biochar

Kaikai Zhang, Peng Sun, Yanrong Zhang

期刊论文

Thermoresponsive block copolymer supported Pt nanocatalysts for base-free aerobic oxidation of 5-hydroxymethyl

期刊论文

Influence of the filler materials on flux-free brazing of pure aluminium (1050)

Kirsten BOBZIN, Lidong ZHAO, Thomas SCHLAEFER, Thomas WARDA,

期刊论文

New perspectives in free nitrous acid (FNA) uses for sustainable wastewater management

期刊论文

Highly selective detection of copper(II) by a “ligand-free” conjugated copolymer in nucleophilic solvents

Weixing Deng, Pengfei Sun, Quli Fan, Lei Zhang, Tsuyoshi Minami

期刊论文

Ionically Imprinting-Based Copper (Ⅱ) Label-Free Detection for Preventing Hearing Loss

Huan Wang, Hui Zhang, Xiaoli Zhang, Hong Chen, Ling Lu, Renjie Chai

期刊论文

Solvent-free mechanochemical mild oxidation method to enhance adsorption properties of chitosan

期刊论文

Design approach for single piston hydraulic free piston diesel engines

Wei WU, Shihua YUAN, Jibin HU, Chongbo JING,

期刊论文

“ALL FREE” — a novel design concept of applying partial oxidation process to vehicle

Ling LIN, Wenshuang LIN, Qingbiao LI, Yao ZHOU,

期刊论文